Jones appeared in the 2010 episode "Amy's Choice", of Doctor Who, as the Dream Lord, and in the Big Finish Productions series' Dark Eyes (audio drama) as Kotris. He also played the role of Samuel Ratchett in Agatha Christie's Poirot TV Series 12 episode "Murder on the Orient Express". In 2011, he played the role of the British spy master Percy Alleline in the adaptation of John Le Carré's Tinker Tailor Soldier Spy and Arnim Zola in Captain America: The First Avenger, a role which he reprised in the sequel Captain America: The Winter Soldier three years later as well as in a cameo in the TV series Agent Carter the following year. In 2012, he had a leading role in the ITV mini-series Titanic, starred as one of the seven dwarves in Snow White and the Huntsman, played Dr. Paul Shackleton in Red Lights, and Max in Virginia. He also portrayed film Director Alfred Hitchcock in the HBO television film The Girl, a role that earned him his first Golden Globe Award nomination, as well as his first Primetime Emmy Award nomination.